Classifications

• • C—CHEMISTRY; METALLURGY
  • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
  • C08F—MACROMOLECULAR COMPOUNDS OBTAINED BY REACTIONS ONLY INVOLVING CARBON-TO-CARBON UNSATURATED BONDS
  • C08F297/00—Macromolecular compounds obtained by successively polymerising different monomer systems using a catalyst of the ionic or coordination type without deactivating the intermediate polymer
  • C08F297/02—Macromolecular compounds obtained by successively polymerising different monomer systems using a catalyst of the ionic or coordination type without deactivating the intermediate polymer using a catalyst of the anionic type
  • C08F297/04—Macromolecular compounds obtained by successively polymerising different monomer systems using a catalyst of the ionic or coordination type without deactivating the intermediate polymer using a catalyst of the anionic type polymerising vinyl aromatic monomers and conjugated dienes
  • C08F297/042—Macromolecular compounds obtained by successively polymerising different monomer systems using a catalyst of the ionic or coordination type without deactivating the intermediate polymer using a catalyst of the anionic type polymerising vinyl aromatic monomers and conjugated dienes using a polyfunctional initiator
• • C—CHEMISTRY; METALLURGY
  • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
  • C08F—MACROMOLECULAR COMPOUNDS OBTAINED BY REACTIONS ONLY INVOLVING CARBON-TO-CARBON UNSATURATED BONDS
  • C08F8/00—Chemical modification by after-treatment
  • C08F8/04—Reduction, e.g. hydrogenation
• • C—CHEMISTRY; METALLURGY
  • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
  • C08F—MACROMOLECULAR COMPOUNDS OBTAINED BY REACTIONS ONLY INVOLVING CARBON-TO-CARBON UNSATURATED BONDS
  • C08F297/00—Macromolecular compounds obtained by successively polymerising different monomer systems using a catalyst of the ionic or coordination type without deactivating the intermediate polymer
  • C08F297/02—Macromolecular compounds obtained by successively polymerising different monomer systems using a catalyst of the ionic or coordination type without deactivating the intermediate polymer using a catalyst of the anionic type
  • C08F297/04—Macromolecular compounds obtained by successively polymerising different monomer systems using a catalyst of the ionic or coordination type without deactivating the intermediate polymer using a catalyst of the anionic type polymerising vinyl aromatic monomers and conjugated dienes
• • C—CHEMISTRY; METALLURGY
  • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
  • C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
  • C08J5/00—Manufacture of articles or shaped materials containing macromolecular substances
  • C08J5/18—Manufacture of films or sheets
• • C—CHEMISTRY; METALLURGY
  • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
  • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
  • C08L23/00—Compositions of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Compositions of derivatives of such polymers
  • C08L23/02—Compositions of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Compositions of derivatives of such polymers not modified by chemical after-treatment
  • C08L23/10—Homopolymers or copolymers of propene
• • C—CHEMISTRY; METALLURGY
  • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
  • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
  • C08L53/00—Compositions of block copolymers containing at least one sequence of a polymer obtained by reactions only involving carbon-to-carbon unsaturated bonds; Compositions of derivatives of such polymers
• • C—CHEMISTRY; METALLURGY
  • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
  • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
  • C08L53/00—Compositions of block copolymers containing at least one sequence of a polymer obtained by reactions only involving carbon-to-carbon unsaturated bonds; Compositions of derivatives of such polymers
  • C08L53/02—Compositions of block copolymers containing at least one sequence of a polymer obtained by reactions only involving carbon-to-carbon unsaturated bonds; Compositions of derivatives of such polymers of vinyl-aromatic monomers and conjugated dienes
  • C08L53/025—Compositions of block copolymers containing at least one sequence of a polymer obtained by reactions only involving carbon-to-carbon unsaturated bonds; Compositions of derivatives of such polymers of vinyl-aromatic monomers and conjugated dienes modified
• • C—CHEMISTRY; METALLURGY
  • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
  • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
  • C08L2205/00—Polymer mixtures characterised by other features
  • C08L2205/03—Polymer mixtures characterised by other features containing three or more polymers in a blend
  • C08L2205/035—Polymer mixtures characterised by other features containing three or more polymers in a blend containing four or more polymers in a blend
• • C—CHEMISTRY; METALLURGY
  • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
  • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
  • C08L23/00—Compositions of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Compositions of derivatives of such polymers
  • C08L23/02—Compositions of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Compositions of derivatives of such polymers not modified by chemical after-treatment
  • C08L23/04—Homopolymers or copolymers of ethene
  • C08L23/08—Copolymers of ethene
  • C08L23/0807—Copolymers of ethene with unsaturated hydrocarbons only containing more than three carbon atoms
  • C08L23/0815—Copolymers of ethene with aliphatic 1-olefins
• • C—CHEMISTRY; METALLURGY
  • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
  • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
  • C08L23/00—Compositions of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Compositions of derivatives of such polymers
  • C08L23/02—Compositions of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Compositions of derivatives of such polymers not modified by chemical after-treatment
  • C08L23/16—Elastomeric ethene-propene or ethene-propene-diene copolymers, e.g. EPR and EPDM rubbers
• • C—CHEMISTRY; METALLURGY
  • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
  • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
  • C08L53/00—Compositions of block copolymers containing at least one sequence of a polymer obtained by reactions only involving carbon-to-carbon unsaturated bonds; Compositions of derivatives of such polymers
  • C08L53/02—Compositions of block copolymers containing at least one sequence of a polymer obtained by reactions only involving carbon-to-carbon unsaturated bonds; Compositions of derivatives of such polymers of vinyl-aromatic monomers and conjugated dienes

Definitions

• the present invention relates to a hydrogenated block copolymer and a composition thereof. More specifically, a hydrogenated block copolymer characterized by being able to impart excellent balance of impact resistance, brittleness temperature, tensile elongation at break, heat deformation resistance, and rigidity to a polypropylene resin, and a polypropylene-based copolymer thereof. It relates to a resin composition. Background art
• Polypropylene-based resin compositions are generally used widely in machine parts, automobile parts, and the like because of their excellent chemical resistance and mechanical properties. Recently, polypropylene resin compositions with excellent impact resistance, brittleness temperature, rigidity, heat deformation resistance, and tensile elongation at break have been pursued in pursuit of functionality and economics of various products, resulting in larger and thinner products.
• the tensile elongation at break is designed to prevent the fragments from scattering at the time of impact fracture when used as an automotive material, to absorb the impact by deformation, or not to break at the time of creep deformation. This is one of the highly demanded physical properties for reasons such as reasons.
• Thermal deformation resistance is also one of the highly required physical properties because the molding material does not deform under the high temperature atmosphere when automotive exterior materials are painted online. These embrittlement temperature, tensile elongation at break, impact resistance and stiffness, and heat deformation resistance are contradictory properties such that when one is improved, the other is worsened, there is a need for an invention that improves the overall balance of physical properties. I was
• Japanese Patent Application Laid-Open No. 3-188114 discloses that the heat of crystal fusion is 8 ca 1 / g or less, which comprises a polymer block composed of a vinyl aromatic compound and a hydrogenated isoprene-butadiene block. Block copolymers are disclosed.
• the present invention requires that the amount of 1,2 bonds be 35% or less, which is particularly The tensile elongation at break deteriorates.
• there is no description or suggestion about the relationship between the heat of crystal fusion and the embrittlement temperature of the composition and no description or suggestion of the order-disorder transition temperature and the thermal deformation resistance of the composition. Therefore, the disclosed technology cannot achieve the purpose of the present invention.
• POLYMER, Volume 38, Number 17 describes a hydrogenated block copolymer consisting of polystyrene and hydrogenated polyphenylene, with a 1,2 bond content of 50 mol% and a styrene content of 50%. Is 20 wt%, the heat of crystal fusion is 5. l J / g, the amount of two bonds is 40 mol%, the amount of styrene is 20 wt%, and the heat of crystal fusion is 12.3 J / g. This paper describes the mechanical properties of these hydrogenated block copolymers, but does not describe any of the effects when used in compositions.
• JP-A-8-20684 discloses crystalline propylene and two types of hydrogenated block copolymers (styrene-ethylene / butylene copolymer) as resin compositions having excellent rigidity, heat deformation resistance, impact resistance, and moldability.
• a resin composition comprising a styrene copolymer, a styrene-ethylene / propylene copolymer), an ethylene-propylene copolymer rubber, and talc is disclosed.
• talc ethylene-propylene copolymer rubber
• a hydrogenated block copolymer capable of imparting an excellent balance of impact resistance, brittleness temperature, tensile elongation at break, heat deformation resistance, and rigidity, and a polypropylene-based resin composition having an excellent balance of these physical properties At present, no product has been obtained.
• An object of the present invention is to provide a polypropylene resin composition that has an excellent balance of impact resistance, brittle temperature, tensile elongation at break, rigidity, and heat deformation resistance, and is also economical. To provide a hydrogenated block copolymer.
• Another object of the present invention is to provide a polypropylene-based resin composition having the above excellent physical property balance. Disclosure of the invention
• a specific hydrogenated block copolymer effectively solves the above problems, and have completed the present invention. That is, it was discovered that a specific hydrogenated block copolymer enables the supply of a composition having an excellent balance of impact resistance, embrittlement temperature, rigidity, heat deformation resistance, and bow I tension elongation at break. It depends.
• the hydrogenated block copolymer of the present invention is mainly composed of a polymer block A mainly composed of two vinyl aromatic hydrocarbon compound monomer units and one hydrogenated hydrogenated monomer unit. 90% or more of the olefinic unsaturated double bonds in the polymer block mainly composed of the hydrogen monomer unit before hydrogenation were hydrogenated.
• the binding amount of the vinyl aromatic hydrocarbon compound in the hydrogenated block copolymer is more than 13% by weight and less than 25% by weight, and the butadiene monomer before hydrogenation is added.
• the amount of 1, 2 bonds in the polymer block mainly composed of units is more than 40 mol% and less than 60 mol%, the heat of crystal fusion ( ⁇ ) is less than 0.05 J / g, The single-disorder transition temperature is 200 ° C or higher, and Hydrogenation with a melt flow rate (MFR) of 0.1 g / 10 min or more and less than 30 g / 10 min under the conditions of a temperature of 230 ° C and a load of 2.16 Kg It is a block copolymer.
• MFR melt flow rate
• the present inventors have newly added a hydrogenated block in which the amount of 1,2 bonds in the polymer block mainly composed of butadiene monomer units before hydrogenation is less than 60 mol%, and furthermore, crystals are eliminated. Further studies were carried out based on the new idea that the composition using a polymer greatly improved the balance of mechanical properties. As a result, it is surprising that the hydrogenated block copolymer which has no crystal component or has a heat of crystal fusion less than a certain value in the 1 to 2 bond amount region of 40 to 60 mol% which originally has crystals. DISCLOSURE OF THE INVENTION The present inventors have found that the present invention significantly improves the physical property balance of the composition, and have been completed.
• the polypropylene resin composition of the present invention comprises (1) 99 to 60 parts by weight of a polypropylene resin, and (2) 1 to 40 parts by weight of the above hydrogenated block copolymer.
• FIG. 1 shows the method of determining the TQDT of SEBS 4.
• FIG. 2 shows a method of determining the TQDT of SEBS11 .
• the hydrogenated block copolymer according to the first embodiment of the present invention comprises a polymer block A mainly composed of two vinyl aromatic hydrocarbon compound monomer units and one hydrogenated butadiene monomer. It is composed of a polymer block B mainly composed of monomer units.
• the monomer unit of the vinyl aromatic conjugate include alkylstyrenes such as styrene, monomethylstyrene, p-methylstyrene and p-butyl styrene, and p-methoxystyrene and vinylnaphthalene.
• alkylstyrenes such as styrene, monomethylstyrene, p-methylstyrene and p-butyl styrene, and p-methoxystyrene and vinylnaphthalene.
• styrene is particularly preferred.
• the content of the monomer unit of the vinyl aromatic compound in the block copolymer is more than 13% by weight and less than 25% by weight. From the viewpoint of the degree, it is preferably from 15% by weight to less than 23% by weight, and particularly preferably from 15% by weight to less than 20% by weight. If the content is 13% by weight or less, the rigidity is deteriorated, and if the content is 25% by weight or more, the embrittlement temperature increases.
• the content of vinyl aromatic monomer units can be measured by a nuclear magnetic resonance apparatus (NMR), an ultraviolet spectrophotometer (UV), or the like.
• the word “mainly” means, for example, "mainly a vinyl aromatic compound monomer unit", a case where one or more kinds of vinyl aromatic monomers are used, or a living room with these. This includes the case where other monomers that undergo anion polymerization are copolymerized. Examples of these other copolymerizable monomers include a co-gen compound monomer, methacrylic acid esters such as methyl methacrylate and butyl methyl acrylate, cyclohexadiene, and force prolactone.
• the form of copolymerization may be any form such as random, alternating, or tapered.
• the two polymer blocks A may have different compositions, molecular weights, and the like.
• the polymer block mainly composed of butadiene monomer units can be arbitrarily selected in the microstructure of the block, and the amount of 1,2 bonds exceeds 40 mol% and exceeds 60 mol%. %, Preferably from 41 mol% to 55 mol%, more preferably from 46 mol% to 54 mol%. If it is less than 40 mol%, poor elongation will result due to poor dispersion, and if it is more than 60 mol%, the brittleness temperature and the heat deformation resistance will deteriorate. In addition, it is desirable that the 1,2 bonds exist as uniformly as possible in the polymer chain (so that the 1,2 bonds do not collect locally).
• the microstructure can be measured by nuclear magnetic resonance (NMR).
• butadiene monomer units includes the case where a butadiene monomer and another monomer that undergoes living anion polymerization are copolymerized.
• These other copolymerizable monomers include other conjugated diene compound monomers such as isoprene, vinyl aromatic compound monomers, methyl methacrylates such as methyl methacrylate and butyl methacrylate, and cyclohexadiene. And force prolactone.
• the form of copolymerization may be any form such as random, alternating, or tapered.
• the term "mainly" means that the corresponding monomer unit is at least more than 50 mol%, preferably at least 70 mol%, more preferably at least 80%, in the polymer block. Especially preferably, it means that it accounts for 90% or more.
• the hydrogenated block copolymer of the present invention 90% or more of the olefinic unsaturated double bonds in the polymer block B before hydrogenation are hydrogenated. If it is less than 90%, the adhesiveness at the polypropylene interface is reduced, the impact resistance and elongation are reduced, and deterioration is caused by heat, light, etc., and the thermoplasticity is reduced. Further, the unsaturated double bond of the benzene ring of the vinyl aromatic compound in the block A may be hydrogenated up to 20% of the entire vinyl aromatic compound.
• the hydrogenation rate can be measured by nuclear magnetic resonance (NMR).
• melt flow rate (M.FR) determined under the conditions of a temperature of 230 °, a load of 2.16 Kg and a melt flow rate (M.FR) of 0.1 g / 10 min according to JISK 7210 (1976 version) of hydrogenated block copolymer Must be in the range of at least 30 g / 10 min.
• a preferred range is from 0.1 g / 10 min to 15 g / l and less than 0 min, a more preferred range is from 1.0 Og / 10 min to less than 1 Og / 10 min, and a particularly preferred range is 3.0 g / l g / 10 min or more and less than 8 g / 10 min. If it is less than 0. l g / 10 min, the impact resistance will deteriorate, and if it is more than 30 g / 10 min, elongation will not occur.
• the order-disorder transition temperature of the hydrogenated block copolymer in the present invention is 200 ° C. or higher.
• the heat deformation resistance can be determined by measuring the heat deformation temperature of the injection-molded composition.
• the order-disorder transition temperature is the temperature at which the phase separation state of a hydrogenated block copolymer that separates into two phases, a rubber phase and a constrained phase, near room temperature disappears, and is measured by small-angle X-ray scattering and rheological measurements. Can be determined.
• the dynamic storage modulus (G ') and the loss modulus (G ") are measured at various temperatures within a sufficient shear rate range, and G' is replaced by G Slope of line plotted against ", off It can be determined from the temperature at which the pieces begin to be the same.
• the temperature dependence of G ' can be measured from a high temperature side at a sufficiently low frequency, for example, below 0.1 Hz, and determined from the inflection point that appears at the highest temperature side.
• the hydrogenated block copolymer is prepared, for example, by a method described in JP-B-36-19286, JP-B-43-14979, JP-B-49-36957, etc., in an anionic polymerization initiator in a hydrocarbon solvent.
• organic compounds such as getyl ether and tetrahydrofuran, and tertiary amines such as triethylamine, N, ⁇ , ⁇ ,, ⁇ , and tetramethylethylene diamine.
• the peak temperature of the reactor internal temperature is 85 ° C or less, and the maximum temperature and the minimum temperature in the reactor during polymerization are low. If the temperature difference ( ⁇ ), which is the temperature difference, is 15 ° C or less, the heat of crystal fusion ( ⁇ ) of the finally obtained hydrogenated block copolymer decreases. In order to keep the reactor internal temperature below 85 ° C and the temperature range ( ⁇ ) below 15 ° C, it is necessary to remove the reaction heat by cooling.
• the peak temperature of the reactor temperature is 80 ° C or less, and the temperature range ( ⁇ ) is 10 ° C or less.
• the heat of crystal fusion ( ⁇ ) of the hydrogenated block copolymer is less than 0.05 J / g. If it is more than 0.05 J / g, the brittle temperature of the obtained composition becomes high.
• the heat of crystal fusion ( ⁇ ) is usually determined by the DSC method. Can be
• the hydrogenated block copolymer of the present invention may be modified by an addition reaction with an unsaturated carboxylic acid or a derivative thereof to introduce a functional group.
• a composition comprising:
• the amount of the hydrogenated block copolymer is less than 1 part by weight, the impact resistance t, embrittlement temperature and elongation are poor, and if it exceeds 40 parts by weight, the rigidity is poor. Further, if necessary, a hydrogenated block copolymer obtained by hydrogenating a conjugated diene polymer block different from the hydrogenated block copolymer of the present invention can be used in combination.
• the polypropylene-based resin used in the resin composition of the present invention is mainly composed of propylene, and, if necessary, ethylene, a monoolefin having 4 to 12 carbon atoms, for example, 1-butene, 1-octene, isobutylene A resin obtained by polymerizing with at least one monomer selected from -1,4-methyl-1-pentene, etc., among which propylene homopolymer, propylene block copolymer, propylene random copolymer, and These include these mixtures, and may be a mixture of different molecular weights and compositions. Particularly preferred is a propylene block copolymer.
• comonomers other than propylene include monoolefins and ethylene.
• ethylene is preferable, and the content of propylene in these copolymers is preferably 55 mol% or more.
• a homopropylene block is used as a continuous phase and an ethylene / monoolefin block forms a dispersed phase. Is preferably 5 to 30% by weight of the propylene block copolymer. This dispersed phase may contain polyethylene.
• melt flow rate of the polypropylene resin in the present invention is preferably in the range of 0.1 to 200 g / 10 minutes. More preferably, it is 50 g / 10 minutes or more in terms of rigidity and moldability.
• melt flow rate of at least one polypropylene resin is 50/10 minutes or more in terms of rigidity and moldability.
• the method of polymerizing the polypropylene resin may be any of conventionally known methods, including transition polymerization, radical polymerization, ionic polymerization and the like.
• the ethylene mono-olefin copolymer rubber may be any copolymer of ethylene and a polyolefin having 3 to 12 carbon atoms, such as propylene, 1-butene, isobutylene, and octene. From the viewpoint of rigidity, an ethylene-octene copolymer is preferred.
• the amount of monoolefin is preferably 15 wt% or more, and an ethylene-octene copolymer having an octene content of 15 wt% or more is preferable because of excellent embrittlement temperature and rigidity.
• the specific gravity of the ethylene monoolefin copolymer is preferably 0.880 g / cc or less, because it is excellent in embrittlement temperature and rigidity.
• These ethylene-monoolefin copolymers are not particularly limited to a polymerization method, but are preferably those obtained by polymerization with a meta-mouth catalyst having a uniform active site because of its low specific gravity.
• the polymerization system may be a solution homogeneous system or a slurry system.
• the inorganic filler includes calcium carbonate, talc, magnesium hydroxide, myriki, barium sulfate, silicic acid (white carbon), titanium oxide, and carbon black.
• the polypropylene composition of the present invention may contain a stabilizer, a lubricant, a coloring agent, a silicone oil, a flame retardant and the like.
• the stabilizer include a hindered phenol-based antioxidant, a phosphorus-based heat stabilizer, a hindered amine-based light stabilizer and a benzotriazole-based UV absorber.
• the lubricant include stearic acid, stearic acid ester, a metal salt of stearic acid, amorphous silica, talc, and my power.
• the polypropylene-based resin composition of the present invention can be adjusted by an apparatus generally used for mixing a high-molecular substance according to the composition ratio of each component.
• mixing devices examples include kneading devices such as Banbury mixers, Labo Plastomill, single-screw extruders, and twin-screw extruders.
• kneading devices such as Banbury mixers, Labo Plastomill, single-screw extruders, and twin-screw extruders.
• the melt-mixing method using an extruder is preferred in terms of productivity and good kneading.
• MFR Conforms to the JIS K7210 L condition.
• Izod impact strength Measured with notch according to JIS K7110.
• Embrittlement temperature Based on JIS K 7216.
• Flexural modulus JIS K 7203 Compliant with a bending speed of 2 mm / min.
• Heat deformation temperature Based on JISK 7207 load 0.45MPa.
• PP1 (MK755H MFR 63 g / 10 min, manufactured by Nippon Polyolefin Co., Ltd.) and PP2 (MK711H MFR 43 g / 10 min, manufactured by Nippon Polyolefin Co., Ltd.), which are propylene block copolymers, were used.
• the heat of crystal fusion was obtained by measuring the DSC carp at a heating rate of 10 ° C / min using a 7 Series Thermal Analysis System manufactured by PEMIN-ELMER, and determining the peak area.
• a sample of the hydrogenated block copolymer for DSC carp measurement a sample which had sufficiently promoted crystallization after melt molding was used.
• the styrene content was measured with an ultraviolet spectrophotometer (UV), the 1,2 bond amount, and the hydrogenation rate was measured with a nuclear magnetic resonance device (N (MR).
• UV ultraviolet spectrophotometer
• N nuclear magnetic resonance device
• the order-disorder transition temperature ( T0DT ) was measured using a RMS 800 mechanical spectrum meter manufactured by Rheometrics, 25 mm parallel plate, from 0.1 rad / sec: 230 ° C under the condition of I 00 rad / sec. G,, and G "were measured at each temperature in the order of C and 200 ° C.
• TaDT was determined to be less than 200 ° C.
• T 0DT was determined to be 200 ° C or more and less than 230 ° C. If the slope was gentle at 200 and 230 ° C, the T QDT was judged to be 230 ° C or higher.
• the MFR was high, it flowed out of the parallel plate during the measurement, making observation impossible.
• the amount of styrene was low, TODT was not clearly observed due to the problem of sensitivity, and it was impossible to observe.
• Figures 1 and 2 show how to determine DT .
• Table 1 shows the structure and analysis values of each sample.
• ENGAGE EG8150 ethylene-octene copolymer with an octene content of 25 wt% and a specific gravity of 868 g / cc manufactured by Dow Plastics, EP07P with a propylene content of 27 wt% and a specific gravity of 0.860 g / cc (produced by Nippon Synthetic Rubber Co., Ltd.) (Ethylene-propylene copolymer).
• Each component (1), component (2), component (3) and component (4) are dry blended in the proportions shown in Table 2, and the resulting mixture is co-axially twin-screw extruded at 230 ° C.
• the mixture was melted and kneaded with a machine (screw diameter 3 Omm) to form pellets.
• the pellets were subjected to injection molding using an injection molding machine set at 230 ° C to prepare test specimens for measurement.
• Table 2 shows the measurement results of the physical properties of the obtained test pieces. Table 2 clearly shows that the resin composition of the present invention is excellent.
• SEBS 1 Water 3 ⁇ 4addition SEBS 1 SEBS 2 SEBS 3 SEBS 4 S EB S 5 SEBS 6 SEBS 7 SEBS 8 SEBS 9 SEBS10 S F.BS 1 sens 11 block 8 fflj 8 fiber 8 dragon 8ffl—ffi 8 ffiffi 8 ffiJiii 'il! 8ffl 18 parts 8 Hiffl part 8 Contract ⁇ Part 8 part 8 Dragon ⁇ ' ⁇ 8 i IU!' ⁇
• the hydrogenated block copolymer of the present invention when formed into a composition, has an excellent balance of impact resistance, embrittlement temperature, tensile elongation at break, rigidity, and heat deformation resistance. Due to these effects, they can be suitably used as automotive interior materials, automotive exterior materials, tubes, various containers, sheets, and the like.

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• 1999
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